Issue 32, 2023

Elucidating the oxygen reduction reaction kinetics on defect engineered nanocarbon electrocatalyst: interplay between the N-dopant and defect sites

Abstract

The active sites of electrocatalysts play a crucial role in the material design and mechanistic exploration of an electrocatalytic reaction. Defect-tailored heteroatom-doped carbon-based electrocatalysts for oxygen reduction reaction (ORR) have been much explored, but there is ambiguity in the prediction of active sites responsible for the performance of the material. To find the origin of the activity of this class of catalysts towards ORR, in this work, we use the quantum mechanics/machine learning (QM/ML) approach to derive energy-optimized models with both N-atoms and 5-8-5 defect sites which manifest exemplary ORR activity. Following this approach, we synthesized defect-engineered graphene (DG) using the zinc template method at 1050 °C to achieve optimum N-dopants and intrinsic (5-8-5) defects. The obtained electrocatalyst exhibits hierarchical porosity, high surface area, low nitrogen content, good stability and a satisfying ORR performance with a half-wave potential (E1/2) of 0.82 V, comparable to that of commercial Pt/C (E1/2 = 0.82 V). Further, the full energy profile was deduced using density functional theory and the charge redistribution in the material cross-verified a reduced overpotential for ORR. This work provides a strategy for the synthesis of noble-metal-free high-performance electrocatalysts for energy conversion.

Graphical abstract: Elucidating the oxygen reduction reaction kinetics on defect engineered nanocarbon electrocatalyst: interplay between the N-dopant and defect sites

Supplementary files

Article information

Article type
Paper
Submitted
14 Ақп. 2023
Accepted
06 Сәу. 2023
First published
07 Сәу. 2023

J. Mater. Chem. A, 2023,11, 17045-17055

Elucidating the oxygen reduction reaction kinetics on defect engineered nanocarbon electrocatalyst: interplay between the N-dopant and defect sites

S. Bhardwaj, S. Kapse, S. Dan, R. Thapa and R. S. Dey, J. Mater. Chem. A, 2023, 11, 17045 DOI: 10.1039/D3TA00871A

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements